Mg, Al-hydrotalcite nanocrystalline was synthesized by the liquid reaction method. And Mg, Al-hydrotalcite/polyethylene(PE) flame-retardant nanocomposites were prepared by co-mixing method at atmospheric pressure. Mg, Al-hydrotalcite nanocrystalline was firstly modified to improve its distribution in polyethylene medium. Based on the mechanical and flame-retardant test results, the effect of the surface treatment agents on the Mg, Al-hydrotalcite/PE nanocomposites was investigated; and it is found that the anion surface active agent is better than other surface treatment agents. Moreover, the effect of pH value on Mg, Al-hydrotalcite/PE nanocomposites was also studied. And it is found that the lower the pH value (from 9.5 to 12.5) is, the better the mechanical and flame-retardant properties of the Mg, Al-hydrotalcitc/PE nanocomposites are. Besides, XRD, SEM and TEM analysis results show that Mg, Al-hydrotalcite nanocrystalline grains distribute evenly throughout the polyethylene organic medium; and part of polyethylene molecules intercalate Mg, Al-hydrotalcite middle layer. Finally, the flame-retardant test results of the inorganic/PE composites show that Mg, Al-hydrotalcite flame-retardant agent is better than Al(OH)(3) flame-retardant agent.